Heterostructures based on layering of two-dimensional (2D) materials such as graphene and hexagonal boron nitride represent a new class of electronic devices. Realizing this potential, however, depends critically on the ability to make high-quality electrical contact. Here, we report a contact geometry in which we metalize only the 1D edge of a 2D graphene layer. In addition to outperforming conventional surface contacts, the edge-contact geometry allows a complete separation of the layer assembly and contact metallization processes. In graphene heterostructures, this enables high electronic performance, including low-temperature ballistic transport over distances longer than 15 micrometers, and room-temperature mobility comparable to the theoretical phonon-scattering limit. The edge-contact geometry provides new design possibilities for multilayered structures of complimentary 2D materials.
SrTiO 3. Whereas in oxygen-deficient SrTiO 3−x and Nb-doped SrTiO 3 films the Hall constant increases markedly below 100 K (29), it is less temperature dependent in LaAlO 3 /SrTiO 3 hetero-structures. In addition, the upper critical field of the heterostructures is an order of magnitude smaller than that of Nb-SrTiO 3 with the same T c. Finally, our observation of both superconducting and insulating behavior on the same sample, depending on the precise LaAlO 3 layer thickness, is very hard to reconcile with a pure oxygen vacancy scenario. Magnetic anisotropy allows magnets to maintain their direction of magnetization over time. Using a scanning tunneling microscope to observe spin excitations, we determined the orientation and strength of the anisotropies of individual iron and manganese atoms on a thin layer of copper nitride. The relative intensities of the inelastic tunneling processes are consistent with dipolar interactions, as seen for inelastic neutron scattering. First-principles calculations indicate that the magnetic atoms become incorporated into a polar covalent surface molecular network in the copper nitride. These structures, which provide atom-by-atom accessibility via local probes, have the potential for engineering anisotropies large enough to produce stable magnetization at low temperatures for a single atomic spin.
Recent progress in large-area synthesis of monolayer molybdenum disulphide, a new two-dimensional direct-bandgap semiconductor, is paving the way for applications in atomically thin electronics. Little is known, however, about the microstructure of this material. Here we have refined chemical vapour deposition synthesis to grow highly crystalline islands of monolayer molybdenum disulphide up to 120 μm in size with optical and electrical properties comparable or superior to exfoliated samples. Using transmission electron microscopy, we correlate lattice orientation, edge morphology and crystallinity with island shape to demonstrate that triangular islands are single crystals. The crystals merge to form faceted tilt and mirror twin boundaries that are stitched together by lines of 8- and 4-membered rings. Density functional theory reveals localized mid-gap states arising from these 8-4 defects. We find that mirror twin boundaries cause strong photoluminescence quenching whereas tilt boundaries cause strong enhancement. Meanwhile, mirror twin boundaries slightly increase the measured in-plane electrical conductivity, whereas tilt boundaries slightly decrease the conductivity.
The properties of polycrystalline materials are often dominated by the size of their grains and by the atomic structure of their grain boundaries. These effects should be especially pronounced in two-dimensional materials, where even a line defect can divide and disrupt a crystal. These issues take on practical significance in graphene, which is a hexagonal, two-dimensional crystal of carbon atoms. Single-atom-thick graphene sheets can now be produced by chemical vapour deposition on scales of up to metres, making their polycrystallinity almost unavoidable. Theoretically, graphene grain boundaries are predicted to have distinct electronic, magnetic, chemical and mechanical properties that strongly depend on their atomic arrangement. Yet because of the five-order-of-magnitude size difference between grains and the atoms at grain boundaries, few experiments have fully explored the graphene grain structure. Here we use a combination of old and new transmission electron microscopy techniques to bridge these length scales. Using atomic-resolution imaging, we determine the location and identity of every atom at a grain boundary and find that different grains stitch together predominantly through pentagon-heptagon pairs. Rather than individually imaging the several billion atoms in each grain, we use diffraction-filtered imaging to rapidly map the location, orientation and shape of several hundred grains and boundaries, where only a handful have been previously reported. The resulting images reveal an unexpectedly small and intricate patchwork of grains connected by tilt boundaries. By correlating grain imaging with scanning probe and transport measurements, we show that these grain boundaries severely weaken the mechanical strength of graphene membranes but do not as drastically alter their electrical properties. These techniques open a new window for studies on the structure, properties and control of grains and grain boundaries in graphene and other two-dimensional materials.
A central goal of modern materials physics and nanoscience is control of materials and their interfaces to atomic dimensions. For interfaces between polar and non-polar layers,this goal is thwarted by a polar catastrophe that forces an interfacial reconstruction. In traditional semiconductors this reconstruction is achieved by an atomic disordering and stoichiometry change at the interface, but in multivalent oxides a new option is available: if the electrons can move, the atoms don't have to. Using atomic-scale electron energy loss spectroscopy we find that there is a fundamental asymmetry between ionically and electronically compensated interfaces, both in interfacial sharpness and carrier density. This suggests a general strategy to design sharp interfaces, remove interfacial screening charges, control the band offset, and hence dramatically improving the performance of oxide devices.Oxide thin films have already found a variety of industrial applications ranging from mainstream electronics to niche markets such as high frequency filters. The wide variety of ground states available to the oxide family offers the potential for richer functionality than available with present conventional semiconductors -from piezoelectric resonators to magnetooptical storage. In some cases, atomic-layer control of the growth is possible, presenting new
The large-scale growth of semiconducting thin films forms the basis of modern electronics and optoelectronics. A decrease in film thickness to the ultimate limit of the atomic, sub-nanometre length scale, a difficult limit for traditional semiconductors (such as Si and GaAs), would bring wide benefits for applications in ultrathin and flexible electronics, photovoltaics and display technology. For this, transition-metal dichalcogenides (TMDs), which can form stable three-atom-thick monolayers, provide ideal semiconducting materials with high electrical carrier mobility, and their large-scale growth on insulating substrates would enable the batch fabrication of atomically thin high-performance transistors and photodetectors on a technologically relevant scale without film transfer. In addition, their unique electronic band structures provide novel ways of enhancing the functionalities of such devices, including the large excitonic effect, bandgap modulation, indirect-to-direct bandgap transition, piezoelectricity and valleytronics. However, the large-scale growth of monolayer TMD films with spatial homogeneity and high electrical performance remains an unsolved challenge. Here we report the preparation of high-mobility 4-inch wafer-scale films of monolayer molybdenum disulphide (MoS2) and tungsten disulphide, grown directly on insulating SiO2 substrates, with excellent spatial homogeneity over the entire films. They are grown with a newly developed, metal-organic chemical vapour deposition technique, and show high electrical performance, including an electron mobility of 30 cm(2) V(-1) s(-1) at room temperature and 114 cm(2) V(-1) s(-1) at 90 K for MoS2, with little dependence on position or channel length. With the use of these films we successfully demonstrate the wafer-scale batch fabrication of high-performance monolayer MoS2 field-effect transistors with a 99% device yield and the multi-level fabrication of vertically stacked transistor devices for three-dimensional circuitry. Our work is a step towards the realization of atomically thin integrated circuitry.
To enhance and optimize nanocatalyst performance and durability for the oxygen reduction reaction in fuel-cell applications, we look beyond Pt-metal disordered alloys and describe a new class of Pt-Co nanocatalysts composed of ordered Pt(3)Co intermetallic cores with a 2-3 atomic-layer-thick platinum shell. These nanocatalysts exhibited over 200% increase in mass activity and over 300% increase in specific activity when compared with the disordered Pt(3)Co alloy nanoparticles as well as Pt/C. So far, this mass activity for the oxygen reduction reaction is the highest among the Pt-Co systems reported in the literature under similar testing conditions. Stability tests showed a minimal loss of activity after 5,000 potential cycles and the ordered core-shell structure was maintained virtually intact, as established by atomic-scale elemental mapping. The high activity and stability are attributed to the Pt-rich shell and the stable intermetallic Pt(3)Co core arrangement. These ordered nanoparticles provide a new direction for catalyst performance optimization for next-generation fuel cells.
Atomically thin two-dimensional semiconductors such as MoS 2 hold great promise in electrical, optical, and mechanical devices and display novel physical phenomena. However, the electron mobility of mono-and few-layer MoS 2 has so far been substantially below theoretically predicted limits, which has hampered efforts to observe its intrinsic quantum transport behaviours. Potential sources of disorder and scattering include both defects such as sulfur vacancies in the MoS 2 itself, and extrinsic sources such as charged impurities and remote optical phonons from oxide dielectrics. To reduce extrinsic scattering, here we developed a van der Waals heterostructure device platform where MoS 2 layers are fully encapsulated within hexagonal boron nitride, and electrically contacted in a multi-terminal geometry using gate-tunable graphene electrodes. Magneto-transport measurements show dramatic improvements in performance, including a record-high Hall mobility reaching 34,000 cm 2 /Vs for 6-layer MoS 2 at low temperature, confirming that low-temperature performance in previous studies was limited by extrinsic interfacial impurities rather than bulk defects in the MoS 2 . We also observed Shubnikov-de Haas oscillations for the first time in high-mobility monolayer and few-layer MoS 2 . Modeling of potential scattering sources and quantum lifetime analysis indicate that a combination of short-ranged and long-ranged interfacial scattering limits low-temperature mobility of MoS 2 . 3Following the many advances in basic science and applications of graphene, other twodimensional (2D) materials, especially transition metal dichalcogenides (TMDCs), have attracted significant interest for their fascinating electrical, optical, and mechanical properties [1][2][3][4][5][6][7][8] . Among the TMDCs, semiconducting MoS 2 has been the mostly widely studied: it shows a thicknessdependent electronic band structure 3,5 , reasonably high carrier mobility 1,2,6-9 , and novel phenomena such as coupled spin-valley physics and the valley Hall effect 10-14 , leading to various applications, such as transistors 1,7,15 , memories 16 , logic circuits 17,18 , light-emitters 19 , and photo-detectors 20 with flexibility and transparency 2,21 . However, as for any 2D material, the electrical and optical properties of MoS 2 are strongly affected by impurities and its dielectric environment 1,2,9,22 , hindering the study of intrinsic physics and limiting the design of 2D-material-based devices. In particular, the theoretical upper bound of the electron mobility of monolayer (1L) MoS 2 is predicted to be from several tens to a few thousands at room temperature (T) and exceed 10 5 cm 2 /Vs at low T depending on the dielectric environment, impurity density and charge carrier density [23][24][25] . In contrast, experimentally measured 1L MoS 2 devices on SiO 2 substrates have exhibited room-T two-terminal field-effect mobility that ranges from 0.1 -55 cm 2 /Vs 1,26,27 . This value increases to 15 -60 cm 2 /Vs with encapsulation by highdielectric materials 1...
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